High‐performance thermal insulating aerogels are attractive candidates for thermal protection in extreme environments. However, inorganic aerogels’ brittleness and poor machinability limit their applications, while organic aerogels suffer from severe strength degradation and structural collapse at high temperatures. Herein, for the first time, a thermo‐responsive self‐ceramifiable aerogel is demonstrated with exceptional strengthening and thermal insulation at high temperatures. This aerogel exhibits excellent toughness and processability like polymers under normal conditions but spontaneously transforms into high‐strength semi‐crystalline hard ceramics upon exposure to high temperatures. After prolonged thermal attack at 800 °C, the strength of the aerogels does not decrease but significantly increases several‐fold (from 0.739 to 2.726 MPa). The self‐ceramization behavior and mechanism of the aerogel are illustrated in detail. The unique self‐ceramifiable capacity enables aerogels to provide fire resistance, high‐strength support, and excellent thermal insulation at ultrahigh temperatures. Even with continuous burning at 1300 °C for 60 min, the 15 mm thick aerogel shows low backside temperature below 300 °C, crack‐free overall structure, and invariant porous morphology. This self‐ceramifiable aerogel opens up a new avenue for developing thermal‐protection materials with toughness, machinability, high strength, and thermal insulation in extreme environments.

Thermo‐Responsive Self‐Ceramifiable Robust Aerogel with Exceptional Strengthening and Thermal Insulating Performance at Ultrahigh Temperatures

Harsh-condition protective materials are essential for resisting various types of environmental damage, such as fire, microbes, scratches, and etc. However, integrating multiple protective functions in one transparent flexible material without sacrificing each other remains a formidable challenge. Here, we demonstrate a smart-puffing transparent flexible phosphite-protonated siloxane (PSiP) that simultaneously exhibits excellent fire protection, high-temperature insulation, antibacterial, antimold, and self-healing properties. A facile one-step method is developed to create this microporous PSiP using (3-aminopropyl)triethoxysilane and phosphite via hydrophilic–hydrophobic interaction-driven self-assembly. Notably, PSiP employs an intelligent thermal-responsive self-puffing behavior to achieve high-temperature insulation, effectively blocking 87.8% of 1400 °C heat. The unique dynamic phosphite-protonated siloxane network in PSiP with high transparency (>92% in the visible region) affords self-healing ability as well as potent defense against fire and bacteria (>99% efficiency). Our findings open up a new avenue for developing transparent, flexible, and high-performance multihazard protective materials with potential applications in buildings, windshields, electronics, and beyond. 

Smart Self-Puffing Phosphite-Protonated Siloxane Network Enables Multifunctional Transparent Protection

Nanomaterials have a critical role in functional materials engineering; however, their efficient recycling, durable use, and multifunctional integration remain a huge challenge for sustainable development. Herein, we report multifunctional biophenolic nanospheres that exploit stimuli-responsive reversible assembly based on multiple directional interactions, allowing for closed-loop recycling and durability, even in complex systems of thermosets. The biobased nanospheres can serve long-term in various environments (high temperature, water, acid, surfactant solutions, etc.). By matching disassembly conditions, the nanospheres can be circularly dissociated into precursors, removed from application systems, reassembled, and reused sustainably. The corresponding mechanism is illustrated by experimental characterization and theoretical simulation. We further demonstrate the recycling and durable multifunctional effects of the nanospheres in thermoset foams. The reproducible nanospheres with diverse radical scavenging abilities endow nanocomposites with excellent mechanical enhancement, aging resistance, and durable flame retardancy. This study paves the way for tackling the pressing issue of high-value functional nanomaterial sustainability. 

Recyclable Biophenolic Nanospheres for Sustainable and Durable Multifunctional Applications in Thermosets

Abstract Vehicles operating in space need to withstand extreme thermal and electromagnetic environments in light of the burgeoning of space science and technology. It is imperatively desired to high insulation materials with lightweight and extensive mechanical properties. Herein, a boron–silica–tantalum ternary hybrid phenolic aerogel (BSiTa-PA) with exceptional thermal stability, extensive mechanical strength, low thermal conductivity (49.6 mW m −1 K −1 ), and heightened ablative resistance is prepared by an expeditious method. After extremely thermal erosion, the obtained carbon aerogel demonstrates noteworthy electromagnetic interference (EMI) shielding performance with an efficiency of 31.6 dB, accompanied by notable loading property with specific modulus of 272.8 kN·m kg −1 . This novel design concept has laid the foundation for the development of insulation materials in more complex extreme environments."Image missing" 

Multifunctional Integrated Organic–Inorganic-Metal Hybrid Aerogel for Excellent Thermal Insulation and Electromagnetic Shielding Performance

Cellulose aerogels prepared by the directional freezing method show huge potential in the field of thermal insulation materials, tissue engineering, and building blocks. However, poor mechanical strength and fire resistance limit their application in buildings and engineering. Inspired by the chemical crosslinking of wood cell walls, we propose a sustainable wall-strengthening strategy for robust cellulose aerogels with high mechanical strength, superior thermal insulation, and flame-retardant performance, denoted as nanopolymerised wood. Specifically, oriented cellulose aerogel, prepared from cellulose nanofibers and polyvinyl alcohol, is impregnated with Na2SiO3 solution and then thermally crosslinked to obtain nanopolymerised wood. The cellulose nanofibers served as a supporting skeleton, while polyvinyl alcohol and Na2SiO3 acted as fillers and adhesives, respectively. This combination densifies the pore walls, resulting in an enhanced compressive strength of the nanopolymerised wood to 64.2 MPa. The directional channels with high interfacial thermal resistance lead to a low radial thermal conductivity of 0.027 W·m−1·K−1. Furthermore, the covalently crosslinked silicates provide nanopolymerised wood with outstanding fire-retardant and self-extinguished properties. The biodegradable components, good mechanical properties, superior thermal insulation, and fire-retardant performance of nanopolymerised wood make it a promising material for sustainable buildings and machine envelopes. 

A sustainable pore wall strengthening for strong and fire-retardant nanopolymerised wood

Aerogel coating (AC) is an emerging constructional material to achieve ambitions to reduce our carbon footprint. However, common ACs, which are usually formulated by straightforward filler–matrix composites, suffer from unsatisfying thermal-insulating performance due to the low porosity and polymer intrusion into the filler. These can be solved by applying an easy foaming process to the ACs, where meanwhile the intrusion issue can be relented by particles decoration on the inner surface of bubbles. Herein, an architected foamy AC by melamine polymer and silica aerogel particles is demonstrated as a proof-of-concept. The high-porosity foamy AC can achieve much lower thermal conductivity and less heat release as well as superhydrophobicity and excellent fire resistance. The coating can be air-sprayed on surfaces regardless of the materials and shapes, followed by natural drying. It provides an economical drop-in measure to enhance the energy conservation and fire safety of various buildings. 

Economical Architected Foamy Aerogel Coating for Energy Conservation and Flame Resistance

Nanosheet-coated synthetic wood with enhanced flame-retardancy by vacuum-assisted sonocoating technique

Freeze-casting has been wildly exploited to construct porous ceramics but usually requires costly and demanding freeze-drying (high vacuum, size limit, and supercooled chamber), which can be avoided by the ambient pressure drying (APD) technique. However, applying APD to freeze-cast ceramic based on an aqueous suspension is still challenging due to inert surface chemistry. Herein, a modified APD strategy is developed to improve the drying process of freeze-cast ceramics by exploiting the simultaneous ice etching, ionic cross-linking, and solvent exchange under mild conditions (-10-0 °C, ambient pressure). This versatile strategy is applicable to various ceramic species, metal ions, and freezing techniques. The incorporated metal ions not only enhance liquid-phase sintering, producing ceramics with higher density and mechanical properties than freeze-cast counterparts, but also render customizable coloration and antibacterial property. The cost-/time-efficient APD is promising for mass production and even successive production of large-size freeze-cast ceramics that exceed the size of commercial freeze-dryers.

Ambient Pressure Drying of Freeze-Cast Ceramics from Aqueous Suspension.

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Economical Architected Foamy Aerogel Coating for Energy Conservation and Flame Resistance

Nanosheet-coated synthetic wood with enhanced flame-retardancy by vacuum-assisted sonocoating technique

Ambient Pressure Drying of Freeze-Cast Ceramics from Aqueous Suspension.